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EP0043303A1 - Verfahren zur Isomerisierung und/oder Umlagerung von Polychlorbenzolen - Google Patents

Verfahren zur Isomerisierung und/oder Umlagerung von Polychlorbenzolen Download PDF

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Publication number
EP0043303A1
EP0043303A1 EP81400952A EP81400952A EP0043303A1 EP 0043303 A1 EP0043303 A1 EP 0043303A1 EP 81400952 A EP81400952 A EP 81400952A EP 81400952 A EP81400952 A EP 81400952A EP 0043303 A1 EP0043303 A1 EP 0043303A1
Authority
EP
European Patent Office
Prior art keywords
chr
benzene
formula
carbon atoms
trichloro
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
EP81400952A
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English (en)
French (fr)
Other versions
EP0043303B1 (de
Inventor
Gérard Soula
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Rhone Poulenc Specialites Chimiques
Original Assignee
Rhone Poulenc Specialites Chimiques
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority claimed from FR8014607A external-priority patent/FR2486068A1/fr
Priority claimed from FR8109392A external-priority patent/FR2505817A1/fr
Application filed by Rhone Poulenc Specialites Chimiques filed Critical Rhone Poulenc Specialites Chimiques
Priority to AT81400952T priority Critical patent/ATE4699T1/de
Publication of EP0043303A1 publication Critical patent/EP0043303A1/de
Application granted granted Critical
Publication of EP0043303B1 publication Critical patent/EP0043303B1/de
Expired legal-status Critical Current

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Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C17/00Preparation of halogenated hydrocarbons
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C17/00Preparation of halogenated hydrocarbons
    • C07C17/35Preparation of halogenated hydrocarbons by reactions not affecting the number of carbon or of halogen atoms in the reaction
    • C07C17/358Preparation of halogenated hydrocarbons by reactions not affecting the number of carbon or of halogen atoms in the reaction by isomerisation

Definitions

  • the present invention relates to a process for isomerization and / or rearrangement of polychlorobenzenes. It relates more particularly to a process for the preparation of polychlorobenzenes by rearrangement and / or isomerization of polychlorobenzenes.
  • this publication describes the obtaining, from 1-iodo-2,4-dibromo-benzene, of the mixture containing the 1,3,5 isomer as well as the 1,2,4-tribromo benzene, the tribromo -1.3.5 benzene and bromo-1 diodo-3.5 benzene.
  • This same publication also describes the reaction of NaNH 2 in liquid ammonia with 1-bromo-2,4-dichloro-benzene, iodo-1-bromo-4 chlorobenzene and iodo-1-tribromo-2,4,6 benzene.
  • the method according to the invention achieves this objective and therefore performs a reaction which has never been possible in the prior art.
  • the compound complexing the cation of the alkaline amide and / or the alcoholate is a sequestering agent of formula: N- [CHR 1 -CHR 2 O- (CHR 3 -CHR 4 -O) n R 5 ] 3 (I) in which is not an integer greater than or equal to 0 and less than or equal to about 10 (0 ⁇ n ⁇ 10), R I, R 2, R 3 and R 4 e n-id or different represent a hydrogen atom or an alkyl radical having from 1 to 4 carbon atoms and R 5 represents an alkyl or cycloalkyl radical having from 1 to 12 carbon atoms, a phenyl radical or a radical -C m H 2 m- ⁇ or C m H 2m + 1 - ⁇ -, where m is between 1 and 12 (1 ⁇ m ⁇ 12).
  • the complexing compound is a macrocyclic polyether having 15 to 30 atoms in the ring and consisting of 4 to 10 -OX units in which X is either -CHR 6 -CHR 7 - either -CHR 6 -CHR 8 -CR 9R 7 - 'R 6 , R 7 , R 8 and R 9 identical or different being a hydrogen atom or an alkyl radical having from 1 to 4 carbon atoms, one of X may be -CHR 6 -CHR 8 -CR 9 R 7 - when the units -0-X include the group -O-CHR 6 -CHR 7 -.
  • a mixture of at least two of the complexing compounds defined above is used.
  • the dichlorobenzenes used in the process according to the invention are 1,2-dichloro-benzene, 1,3-dichloro-benzene and 1,4-dichloro-benzene.
  • the trichlorobenzenes concerned are 1,2,3,3-trichloro benzene, 1,2,4,4-trichlorobenzene, and 1,3,5-trichlorobenzene.
  • tetrachlorobenzenes are tetrachloro-1,2,4,5 benzene, tetrachloro-1,2,3,5 benzene and tetrachloro-1,2,3,4 benzene.
  • the invention is based on the fact that a complexing compound forms with the alkaline amide and / or the alkali alcoholate a complex which allows the extraction of a hydrogen from a polychlorobenzene which give a carbanion.
  • This carbanion due to the complexation of the alkaline cation is soluble in the medium which allows it to extract chlorine from another polychlorobenzene molecule, the reaction reproducing according to the same scheme with the other species present in the reaction medium. .
  • the amide or alcoholate anion extracts a hydrogen from the trichlorobtinzene to give the following three carbantons: in variable proportions depending on the acidity of the hydrogen torn off. It is the CI carbanion which will be the majority here, but it will be the CIII carbanion which will be the most reactive in the following stage of pulling out a chlorine atom from the pentachlorobenzene.
  • carbanion CIII on pentachlorobenzene. mainly gives the carbanion: resulting from the tearing of chlorine 3 from pentachlorobenzene (other carbanions are formed by tearing of a chlorine atom on the other sites, but in smaller proportions) and tetrachloro-1,2,3,5:
  • 1,2,4,4-trichloro benzene can be transformed into 1,3,5-trichloro benzene.
  • a tetrachlorobenzene such as' tetrachloro-1,2,4,5 benzene
  • trichloro-1,2,4 benzene under the conditions of the invention, this disappearance is observed. the latter in favor of 1,3,5-trichlorobenzene.
  • a sequestering agent of formula (I) is used in which R 1 , R 2 , R 3 and R 4 represent a hydrogen atom or a methyl radical, R 5 and n having the previous meaning.
  • n is greater than or equal to 0 and less than uu equal to 6 and for which R 5 represents an alkyl radical having from 1 to 4 carbon atoms.
  • the macrocyclic polyethers which can be used in the process according to the invention are known by the general name of "crown ethers" and are described in French patent 69.43879 published under number 2,026,481.
  • crown ethers which can be used according to the invention are:
  • the process according to the invention can be carried out in the presence or in the absence of solvent.
  • it is the starting polychlorobenzene (s) which plays the role of solvent.
  • the latter must meet a certain number of conditions: it must first of all dissolve the sequestering agent (the latter is soluble in most of the usual solvents) and the polychlorobenzenes; it must also be chemically inert with respect to polychlorobenzenes and amide.
  • An aromatic solvent is preferably chosen, such as, for example, chlorobenzene, benzene or toluene.
  • the choice of the sequestering agent most suited to the implementation of the method according to the invention is also made, taking into account the size of the alkali metal cation of the amide.
  • alkali metal amide (s) used in the context of the process according to the invention are chosen from the group comprising NaNH 2 , KNH2 , L i NH2 . We prefer to use NaNH 2 .
  • the alkali alcoholate (s) used in the context of the process according to the invention are chosen from the group comprising the compounds R0 - M + where M + preferably represents Na + and K + and where R represents an alkyl radical preferably containing 1 to 6 carbon atoms. Mention may be made, as an example, of sodium and potassium t-butylates.
  • the method according to the invention is preferably carried out at a temperature between -20 ° C and 60 ° C. Even more preferably, the reaction takes place between 0 and 40 ° C.
  • the sequestering agent is used in an amount such that the molar ratio of the sequestering agent of formula (I) to the alkaline amide is preferably between approximately 0.005 and approximately 0.5. Even more preferably, this ratio is between approximately 0.02 and approximately 0.2.
  • the molar ratio of the alkali amide to the starting polychlorobenzene (s) is preferably between approximately 1 and approximately 0.05. Even more preferably, it is between approximately 0.5 and approximately 0.05.
  • the proportions of the starting polychlorohenzenes, when a mixture of these is used, can vary within wide limits. These proportions are not a critical element of the invention.
  • 1,3,5-trichloro benzene is an intermediate of great importance for the synthesis of compounds with phytosanitary activity which is obtained in the prior art according to delicate and costly implementation methods such as for example, by chlorination of 1-bromo-3,5-dichloro benzene, in the presence of an azobisnitrile compound or a benzoyl peroxide (Japanese patent application 78.18797).
  • the invention therefore also relates to an isomerization and / or rearrangement process as defined above, for the preparation of 1,3,5-trichloro benzene characterized in that the reaction is carried out, at least a tetrachlorobenzene optionally mixed with 1,2,3,3-trichlorobenzene and / or 1,2,4-trichlorobenzene and / or pentachlorobenzene and / or hexachlorobenzene.
  • a mixture of têtrachloro-1,2,4,5 benzene and trichloro-1,2,4 benzene is used.
  • 1,2,4,5-tetrachloro benzene and 1,2,4-trichloro benzene are used in amounts such that the molar ratio of tetrachloro to trichloro is between approximately 0.1 and approximately 10.
  • the polychlorobenzene mixture obtained at the end of the reaction is separated according to techniques well known to those skilled in the art, for example by distillation and / or fractional crystallization.
  • the sequestering agents of formula (I) used in the process according to the invention can be prepared as described in the French patent application published under the number 2.450.120.
  • tetrachlorobenzene 1 2 4 5 or 21.8 g 0.1 mol of tetrachlorobenzene 1 2 4 5 or 21.8 g is then introduced under nitrogen (anhydrous) into a 250 ml reactor equipped with a condenser and a magnetic stirrer, followed by making up to 100 g with anhydrous chlorobenzene .
  • the mixture is stirred and cooled to 15 ° C.
  • 0.005 mole of tris (3.6-dioxa heptyl) amine is then added, ie 1.6 g and 3.9 g of a mixture of sodium amide in toluene (50% - 50%), or approximately 0.05 mole of sodium amide.
  • Example No. 1 Under the operating conditions used in Example No. 1, 0.1 mol of tetrachlorobtenzene-1,2,3,4, or 21.8 g, is introduced under nitrogen, then it is made up to 100 g with anhydrous chlorobenzene. 0.005 mole of tris (dioxa-3.6 heptyl) amine is added, ie 1.6 g and 2 g of sodium amide in solution in toluene. An increase in temperature is observed from 19 ° C to 25 ° C. After 2 h of reaction, with stirring, the composition of the polychlorobenzenes is as follows:
  • the mixture is stirred at room temperature of 18 ° C.
  • crown ether "Dicyclohexyl 18 C-6" of formula: or 0.93 g and a me Lange of sodium amide in toluene (50% - 50%) or about 0.02 mole of sodium amide.
  • the mixture is stirred at room temperature of 19 ° C.
  • a temperature of 17 ° C is maintained for 2 hours.
  • reaction mixture is then taken up in 200 ml of water and 50 ml of dichloromethane.
  • organic layer is then analyzed:

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
EP81400952A 1980-07-01 1981-06-16 Verfahren zur Isomerisierung und/oder Umlagerung von Polychlorbenzolen Expired EP0043303B1 (de)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AT81400952T ATE4699T1 (de) 1980-07-01 1981-06-16 Verfahren zur isomerisierung und/oder umlagerung von polychlorbenzolen.

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
FR8014607A FR2486068A1 (fr) 1980-07-01 1980-07-01 Procede d'isomerisation et/ou de rearrangement de polychlorobenzenes
FR8014607 1980-07-01
FR8109392A FR2505817A1 (fr) 1981-05-12 1981-05-12 Procede d'isomerisation et/ou de rearrangement de polychlorobenzenes
FR8109392 1981-05-12

Publications (2)

Publication Number Publication Date
EP0043303A1 true EP0043303A1 (de) 1982-01-06
EP0043303B1 EP0043303B1 (de) 1983-09-21

Family

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Family Applications (1)

Application Number Title Priority Date Filing Date
EP81400952A Expired EP0043303B1 (de) 1980-07-01 1981-06-16 Verfahren zur Isomerisierung und/oder Umlagerung von Polychlorbenzolen

Country Status (3)

Country Link
US (1) US4629815A (de)
EP (1) EP0043303B1 (de)
DE (1) DE3160950D1 (de)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4479022A (en) * 1981-04-08 1984-10-23 Rhone-Poulenc Specialites Chimiques Isomerization of bromohalogenobenzenes

Families Citing this family (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB8716587D0 (en) * 1987-07-14 1987-08-19 Shell Int Research Preparing thiophene derivatives
US5030777A (en) * 1989-10-31 1991-07-09 Standard Chlorine Of Delaware, Inc. Synthesis of 3,5-dichloroalkylbenzene and recovery of 1,3-dichlorobenzene
JPH04112843A (ja) * 1990-09-03 1992-04-14 Toray Ind Inc トリクロルベンゼンの異性化方法
US5235020A (en) * 1991-12-31 1993-08-10 Amoco Corporation Process for preparation of poly(aryl ether) polymers by acyclic catalysts
CN101891587B (zh) * 2010-07-19 2012-05-23 扬州大学 间三氯苯的制备方法

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1061506A (fr) * 1951-10-04 1954-04-13 Union Carbide & Carbon Corp Isomérisation des dichlorobenzènes
US2866829A (en) * 1956-03-26 1958-12-30 Woodruff Douglas Isomerization of polychlorobenzenes

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2355337A (en) * 1942-08-28 1944-08-08 Rohm & Haas Preparation of ether amines
FR2459216A1 (fr) * 1979-06-20 1981-01-09 Rhone Poulenc Ind Procede de preparation d'ethers aryliques

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1061506A (fr) * 1951-10-04 1954-04-13 Union Carbide & Carbon Corp Isomérisation des dichlorobenzènes
US2866829A (en) * 1956-03-26 1958-12-30 Woodruff Douglas Isomerization of polychlorobenzenes

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
Journal of the American Chemical Society, Vol. 93, 10 Mars 1971, Easton (US) J.F. BUNNETT et al.: "Isomerization and Disproportionation of Trihalobenzenes Catalyzed by Potassium Analide in Liquid Ammonia", pages 1183-1190 *

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4479022A (en) * 1981-04-08 1984-10-23 Rhone-Poulenc Specialites Chimiques Isomerization of bromohalogenobenzenes

Also Published As

Publication number Publication date
DE3160950D1 (en) 1983-10-27
EP0043303B1 (de) 1983-09-21
US4629815A (en) 1986-12-16

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